Sub-4 nm PtZn Intermetallic Nanoparticles for Enhanced Mass and Specific Activities in Catalytic Electrooxidation Reaction

Qi, Zhiyuan; Xiao, Chaoxian; Liu, Cong; Goh, Tian Wei; Zhou, Lin; Maligal-Ganesh, Raghu; Pei, Yuchen; Li, Xinle; Curtiss, Larry A.; Huang, Wenyu

doi:10.1021/jacs.6b12780

Title: Sub-4 nm PtZn Intermetallic Nanoparticles for Enhanced Mass and Specific Activities in Catalytic Electrooxidation Reaction

Journal Article · Wed Mar 08 00:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b12780· OSTI ID:1355406

Qi, Zhiyuan ^[1]; Xiao, Chaoxian ^[1]; Liu, Cong ^[2];

^[1]; Zhou, Lin ^[3]; Maligal-Ganesh, Raghu ^[1]; Pei, Yuchen ^[1]; Li, Xinle ^[1];

^[4];

^[5]

Iowa State Univ., Ames, IA (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Ames Lab., Ames, IA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Iowa State Univ., Ames, IA (United States). Dept. of Chemistry; Ames Lab., Ames, IA (United States)

Atomically ordered intermetallic nanoparticles (iNPs) have sparked considerable interest in fuel cell applications by virtue of their exceptional electronic and structural properties. However, the synthesis of small iNPs in a controllable manner remains a formidable challenge because of the high temperature generally required in the formation of intermetallic phases. Here in this paper we report a general method for the synthesis of PtZn iNPs (3.2 ± 0.4 nm) on multiwalled carbon nanotubes (MWNT) via a facile and capping agent free strategy using a sacrificial mesoporous silica (mSiO₂) shell. The as-prepared PtZn iNPs exhibited ca. 10 times higher mass activity in both acidic and basic solution toward the methanol oxidation reaction (MOR) compared to larger PtZn iNPs synthesized on MWNT without the mSiO₂ shell. Density functional theory (DFT) calculations predict that PtZn systems go through a “non-CO” pathway for MOR because of the stabilization of the OH* intermediate by Zn atoms, while a pure Pt system forms highly stable COH* and CO* intermediates, leading to catalyst deactivation. Experimental studies on the origin of the backward oxidation peak of MOR coincide well with DFT predictions. Moreover, the calculations demonstrate that MOR on smaller PtZn iNPs is energetically more favorable than larger iNPs, due to their high density of corner sites and lower-lying energetic pathway. Therefore, smaller PtZn iNPs not only increase the number but also enhance the activity of the active sites in MOR compared with larger ones. This work opens a new avenue for the synthesis of small iNPs with more undercoordinated and enhanced active sites for fuel cell applications.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: CHE-1607305; AC02-07CH11358; AC02-06CH11357

OSTI ID:: 1355406

Report Number(s):: IS-J-9261; TRN: US1702295

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 13; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 215 works

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